Design and Performance Evaluation of La–Ce–Zr Oxide-Based and High-Entropy Catalysts for Hydrogen Production via Tri-Reforming

Hydrogen is becoming a central energy carrier in the shift toward low-carbon energy systems. The rising demand for green hydrogen is accelerating the development of more efficient and sustainable production technologies, including methane Tri-Reforming. In this scenario, the development of advanced, stable, and high-performance catalysts is essential to enhance hydrogen competitiveness and facilitate its adoption in different fields of applications. This thesis investigates the synthesis and characterization of catalysts for Hydrogen and Syngas production via methane Tri-Reforming, a process that combines partial oxidation, steam reforming, and dry reforming. The main objective is to develop catalysts capable of maximizing hydrogen and syngas yield for downstream processes while minimizing coke formation. Catalysts were prepared using impregnation and supported deposition methods and characterized through BET, XRD, TPR, Raman Spectroscopy and SEM-EDS to evaluate surface area, crystalline structure, and morphology. Among the synthesized samples, a high-entropy catalyst was also explored to assess the potential of this innovative material class in terms of stability and catalytic activity. Activity tests were conducted in a laboratory-scale plant, monitoring methane conversion, syngas composition and operational stability; reaction products were analyzed by gas chromatography. Results indicate that support choice, active metal dispersion, and compositional complexity significantly influence performance, with Ni-based catalysts on mesoporous supports achieving high methane conversion and resistance to deactivation. These findings suggest that targeted catalyst design, including high-entropy approaches, can enhance the efficiency of methane Tri-Reforming, providing a promising strategy for the sustainable production of syngas for industrial downstream applications like ammonia and biofuels productions.